When Matt met Zooey, it was, naturally, on the set of a movie. They bonded over their love of British singer/songwriter Richard Thompson and decided to make an album. This is how these things generally tend to happen.

“We met on the set of this film ‘The Go-Getter,’ and the director of the movie wanted us to do a duet for the end credits,” Zooey said. “We did a Richard & Linda Thompson song, and that was one of the first things that was exciting about talking to Matt. We had a lot of the same favorite songs and favorite artists, and we admire people that I don’t necessarily bring up in conversations, because most people have no idea what I’m talking about.”

“I had heard Zooey sing before, in ‘Elf,’ and I knew she was a great singer, but I didn’t know she wrote songs,” Matt added. “Because you don’t really expect actors to write great songs, and her songs are incredible. So that was one of the funnest parts of working with her: surprising people.”

OK, so you should probably know that Zooey is actress Zooey Deschanel. Matt is musician M. Ward. They record together under the alias She & Him. Their debut album, the appropriately named Volume One, is a strummy, sunny ode to ’50s country, ’60s pop and ’70s balladry. Deschanel wrote 10 of the album’s 13 songs — tales of lost loves and broken hearts — and delivers them all in a breathy, bellwether-clear voice. Ward heaps on dusty, sun-dappled guitars and filters it all through a gauzy veil of production. The whole thing is w-a-a-a-y better than anything else in the actress-slash-musician canon (we’re looking at you, Scarlett). You have every right to be surprised by that fact.

“Most music on the radio hearkens back to the ’60s and ’70s … mainly older records that have been my biggest inspiration since I started making records,” Ward said. “It turned out that [Zooey and I] grew up listening to a lot of the same records, so it was a fun challenge for me to get those atmospherics across in the production side of things.”

“My favorite songwriters are mostly people that were writing a lot of music in the ’60s and ’70s. People like Carole King and Smokey Robinson. There are oh so many,” Deschanel added. “So I sort of had those as, like, the ultimate songs in the world, in my head, you know? I had those people as the ultimate songwriters, so [the album] was like making a mixtape. Every day, when we were recording, I had, like, a new 80-minute mixtape!”

The duo had originally worked via e-mail — Deschanel wrote all the lyrics and music herself, and would send them to Ward for tinkering — but decided to put the finishing touches on Volume One in Ward’s Portland, Oregon, studio. They released it on North Carolina’s stalwart Merge Records in March, played a series of standing-room-only gigs at the South by Southwest festival in Austin, Texas, and played a handful of shows. And now, despite Deschanel’s busy schedule (she’ll appear in M. Night Shyamalan’s “The Happening” next month), She & Him are already thinking about starting work on Volume Two. After all, this is how these things tend to happen.

“We’re getting the ball rolling,” Ward said. “It’s too early to say, because we’ve just started.”

“I’m just writing some stuff now for Volume Two,” Deschanel added. “We’ve done some demos. We like to work in an improvisational way, so it’ll have its own special personality.”